In this study,the rational construction of Fe^(Ⅲ)-centered porphyrin-based bifunctional ionic porous organic polymers(Fe-IPOP1/2)for a one-step,halogen-free,cascade transformation of olefins and CO_(2) to cyclic carb...In this study,the rational construction of Fe^(Ⅲ)-centered porphyrin-based bifunctional ionic porous organic polymers(Fe-IPOP1/2)for a one-step,halogen-free,cascade transformation of olefins and CO_(2) to cyclic carbonates as compared to the conventional two-step process involving epoxides is presented.The ionic polymers,Fe-IPOP1/2 showed selective and recyclable uptake of CO_(2) with an interaction energy of 32.2/39.6 kJ mol^(-1) signifying the stronger interaction of carbon dioxide with the frameworks.Both the polymers were found to be thermally stable up to 300℃ and exhibited promising catalytic performance in the one-step,halogen-free synthesis of cyclic carbonates under eco-friendly,cocatalyst/solvent-free,atmospheric pressure conditions.The excellent catalytic activity of Fe-IPOP1/2 for a one-pot synthesis of cyclic carbonates has been ascribed to the presence of highly exposed oxophilic Fe^(Ⅲ) sites and nucleophilic Br-anions in the polymers.Notably,this one-pot synthesis strategy was extended for the transformation of various substituted olefins to their respective carbonates in good yield and selectivity.Further,Fe-IPOP1 showed good reusability with retention of catalytic activity for multiple cycles of usage.展开更多
基金the Science&Engineering Research Board(SERB),Department of Science and Technology,Govt.of India,for financial support(CRG/2018/001176).
文摘In this study,the rational construction of Fe^(Ⅲ)-centered porphyrin-based bifunctional ionic porous organic polymers(Fe-IPOP1/2)for a one-step,halogen-free,cascade transformation of olefins and CO_(2) to cyclic carbonates as compared to the conventional two-step process involving epoxides is presented.The ionic polymers,Fe-IPOP1/2 showed selective and recyclable uptake of CO_(2) with an interaction energy of 32.2/39.6 kJ mol^(-1) signifying the stronger interaction of carbon dioxide with the frameworks.Both the polymers were found to be thermally stable up to 300℃ and exhibited promising catalytic performance in the one-step,halogen-free synthesis of cyclic carbonates under eco-friendly,cocatalyst/solvent-free,atmospheric pressure conditions.The excellent catalytic activity of Fe-IPOP1/2 for a one-pot synthesis of cyclic carbonates has been ascribed to the presence of highly exposed oxophilic Fe^(Ⅲ) sites and nucleophilic Br-anions in the polymers.Notably,this one-pot synthesis strategy was extended for the transformation of various substituted olefins to their respective carbonates in good yield and selectivity.Further,Fe-IPOP1 showed good reusability with retention of catalytic activity for multiple cycles of usage.